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Title: Toward an understanding of the increase in enzymatic hydrolysis by mechanical refining

Abstract

Mechanical refining is a low-capital and well-established technology used in pulp and paper industry to improve fiber bonding for product strength. Refining can also be applied in a biorefinery context to overcome the recalcitrance of pretreated biomass by opening up the biomass structure and modifying substrate properties (e.g., morphology, particle size, porosity, crystallinity), which increases enzyme accessibility to substrate and improves carbohydrate conversion. Although several characterization methods have been used to identify the changes in substrate properties, there is no systematic approach to evaluate the extent of fiber cell wall disruption and what physical properties can explain the improvement in enzymatic digestibility when pretreated lignocellulosic biomass is mechanically refined. This is because the fiber cell wall is complex across multiple scales, including the molecular scale, nano- and meso-scale (microfibril), and microscale (tissue level). A combination of advanced characterization tools is used in this study to better understand the effect of mechanical refining on the meso-scale microfibril assembly and the relationship between those meso-scale modifications and enzymatic hydrolysis. Enzymatic conversion of autohydrolysis sugarcane bagasse was improved from 69.6 to 77.2% (11% relative increase) after applying mechanical refining and an increase in enzymatic digestibility is observed with an increase in refining intensity.more » Based on a combination of advanced characterizations employed in this study, it was found that the refining action caused fiber size reduction, internal delamination, and increase in pores and swellability. A higher level of delamination and higher increase in porosity, analyzed by TEM and DSC, were clearly demonstrated, which explain the faster digestibility rate during the first 72 h of enzymatic hydrolysis for disc-refined samples when compared to the PFI-refined samples. Additionally, an increased inter-fibrillar distance between cellulose microfibrils at the nano-meso-scale was also revealed by SFG analysis, while no evidence was found for a change in crystalline structure by XRD and solid-state NMR analysis.« less

Authors:
 [1];  [2];  [3];  [4];  [1];  [2];  [1];  [1]; ORCiD logo [1]
  1. North Carolina State Univ., Raleigh, NC (United States)
  2. Pennsylvania State Univ., University Park, PA (United States)
  3. Brazilian Bioethanol Science and Technology Lab. (CTBE), Campinas, SP (Brazil)
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Bioenergy Technologies Office (BETO)
OSTI Identifier:
1482793
Report Number(s):
NREL/JA-2700-72807
Journal ID: ISSN 1754-6834
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Biotechnology for Biofuels
Additional Journal Information:
Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 1754-6834
Publisher:
BioMed Central
Country of Publication:
United States
Language:
English
Subject:
09 BIOMASS FUELS; sugarcane bagasse; autohydrolysis pretreatment; mechanical refining; enzymatic hydrolysis; fiber morphology; fiber internal delamination; cellulose crystallinity; fiber porosity

Citation Formats

de Assis, Tiago, Huang, Shixin, Driemeier, Carlos Eduardo, Donohoe, Bryon S., Kim, Chaehoon, Kim, Seong H., Gonzalez, Ronalds, Jameel, Hasan, and Park, Sunkyu. Toward an understanding of the increase in enzymatic hydrolysis by mechanical refining. United States: N. p., 2018. Web. doi:10.1186/s13068-018-1289-3.
de Assis, Tiago, Huang, Shixin, Driemeier, Carlos Eduardo, Donohoe, Bryon S., Kim, Chaehoon, Kim, Seong H., Gonzalez, Ronalds, Jameel, Hasan, & Park, Sunkyu. Toward an understanding of the increase in enzymatic hydrolysis by mechanical refining. United States. https://doi.org/10.1186/s13068-018-1289-3
de Assis, Tiago, Huang, Shixin, Driemeier, Carlos Eduardo, Donohoe, Bryon S., Kim, Chaehoon, Kim, Seong H., Gonzalez, Ronalds, Jameel, Hasan, and Park, Sunkyu. Thu . "Toward an understanding of the increase in enzymatic hydrolysis by mechanical refining". United States. https://doi.org/10.1186/s13068-018-1289-3. https://www.osti.gov/servlets/purl/1482793.
@article{osti_1482793,
title = {Toward an understanding of the increase in enzymatic hydrolysis by mechanical refining},
author = {de Assis, Tiago and Huang, Shixin and Driemeier, Carlos Eduardo and Donohoe, Bryon S. and Kim, Chaehoon and Kim, Seong H. and Gonzalez, Ronalds and Jameel, Hasan and Park, Sunkyu},
abstractNote = {Mechanical refining is a low-capital and well-established technology used in pulp and paper industry to improve fiber bonding for product strength. Refining can also be applied in a biorefinery context to overcome the recalcitrance of pretreated biomass by opening up the biomass structure and modifying substrate properties (e.g., morphology, particle size, porosity, crystallinity), which increases enzyme accessibility to substrate and improves carbohydrate conversion. Although several characterization methods have been used to identify the changes in substrate properties, there is no systematic approach to evaluate the extent of fiber cell wall disruption and what physical properties can explain the improvement in enzymatic digestibility when pretreated lignocellulosic biomass is mechanically refined. This is because the fiber cell wall is complex across multiple scales, including the molecular scale, nano- and meso-scale (microfibril), and microscale (tissue level). A combination of advanced characterization tools is used in this study to better understand the effect of mechanical refining on the meso-scale microfibril assembly and the relationship between those meso-scale modifications and enzymatic hydrolysis. Enzymatic conversion of autohydrolysis sugarcane bagasse was improved from 69.6 to 77.2% (11% relative increase) after applying mechanical refining and an increase in enzymatic digestibility is observed with an increase in refining intensity. Based on a combination of advanced characterizations employed in this study, it was found that the refining action caused fiber size reduction, internal delamination, and increase in pores and swellability. A higher level of delamination and higher increase in porosity, analyzed by TEM and DSC, were clearly demonstrated, which explain the faster digestibility rate during the first 72 h of enzymatic hydrolysis for disc-refined samples when compared to the PFI-refined samples. Additionally, an increased inter-fibrillar distance between cellulose microfibrils at the nano-meso-scale was also revealed by SFG analysis, while no evidence was found for a change in crystalline structure by XRD and solid-state NMR analysis.},
doi = {10.1186/s13068-018-1289-3},
journal = {Biotechnology for Biofuels},
number = 1,
volume = 11,
place = {United States},
year = {Thu Oct 25 00:00:00 EDT 2018},
month = {Thu Oct 25 00:00:00 EDT 2018}
}

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Works referenced in this record:

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Cellulose co-crystallization and related phenomena occurring in hydrothermal treatment of sugarcane bagasse
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Enhancement in enzymatic hydrolysis by mechanical refining for pretreated hardwood lignocellulosics
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Production of fermentable sugars from sugarcane bagasse by enzymatic hydrolysis after autohydrolysis and mechanical refining
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Visualizing lignin coalescence and migration through maize cell walls following thermochemical pretreatment
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Dynamic vapor sorption and thermoporometry to probe water in celluloses
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Pretreatment technologies for an efficient bioethanol production process based on enzymatic hydrolysis: A review
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A highly efficient dilute alkali deacetylation and mechanical (disc) refining process for the conversion of renewable biomass to lower cost sugars
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Effects of fibrillation on the wood fibers’ enzymatic hydrolysis enhanced by mechanical refining
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Visualizing lignin coalescence and migration through maize cell walls following thermochemical pretreatment
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  • Biotechnology and Bioengineering, Vol. 101, Issue 5
  • DOI: 10.1002/bit.21959

Mechanistic insights into the liquefaction stage of enzyme-mediated biomass deconstruction
journal, August 2017

  • van der Zwan, Timo; Hu, Jinguang; Saddler, Jack N.
  • Biotechnology and Bioengineering, Vol. 114, Issue 11
  • DOI: 10.1002/bit.26381

Measuring the crystallinity index of cellulose by solid state 13C nuclear magnetic resonance
journal, June 2009


Dynamic vapor sorption and thermoporometry to probe water in celluloses
journal, May 2012


Cellulose co-crystallization and related phenomena occurring in hydrothermal treatment of sugarcane bagasse
journal, April 2015


Reduction of Enzyme Dosage by Oxygen Delignification and Mechanical Refining for Enzymatic Hydrolysis of Green Liquor-Pretreated Hardwood
journal, June 2011

  • Koo, Bon-Wook; Treasure, Trevor H.; Jameel, Hasan
  • Applied Biochemistry and Biotechnology, Vol. 165, Issue 3-4
  • DOI: 10.1007/s12010-011-9301-4

Pretreatment technologies for an efficient bioethanol production process based on enzymatic hydrolysis: A review
journal, July 2010


Synthetic multi-component enzyme mixtures for deconstruction of lignocellulosic biomass
journal, December 2010


Enhancement in enzymatic hydrolysis by mechanical refining for pretreated hardwood lignocellulosics
journal, November 2013


Enzymatic hydrolysis of autohydrolyzed wheat straw followed by refining to produce fermentable sugars
journal, January 2014


Production of fermentable sugars from sugarcane bagasse by enzymatic hydrolysis after autohydrolysis and mechanical refining
journal, March 2015


Use of mechanical refining to improve the production of low-cost sugars from lignocellulosic biomass
journal, January 2016


Effects of fibrillation on the wood fibers’ enzymatic hydrolysis enhanced by mechanical refining
journal, April 2016


Changes in pore size distribution during the drying of cellulose fibers as measured by differential scanning calorimetry
journal, October 2006


Lignin contributions to the nanoscale porosity of raw and treated lignocelluloses as observed by calorimetric thermoporometry
journal, April 2016


Multimodal Broadband Vibrational Sum Frequency Generation (MM-BB-V-SFG) Spectrometer and Microscope
journal, December 2015

  • Lee, Christopher M.; Kafle, Kabindra; Huang, Shixin
  • The Journal of Physical Chemistry B, Vol. 120, Issue 1
  • DOI: 10.1021/acs.jpcb.5b10290

Combined Deacetylation and PFI Refining Pretreatment of Corn Cob for the Improvement of a Two-Stage Enzymatic Hydrolysis
journal, May 2014

  • Zhang, Yuedong; Mu, Xindong; Wang, Haisong
  • Journal of Agricultural and Food Chemistry, Vol. 62, Issue 20
  • DOI: 10.1021/jf500189a

Monitoring Meso-Scale Ordering of Cellulose in Intact Plant Cell Walls Using Sum Frequency Generation Spectroscopy
journal, August 2013


Cellulose crystallinity index: measurement techniques and their impact on interpreting cellulase performance
journal, January 2010

  • Park, Sunkyu; Baker, John O.; Himmel, Michael E.
  • Biotechnology for Biofuels, Vol. 3, Issue 1
  • DOI: 10.1186/1754-6834-3-10

Helically agitated mixing in dry dilute acid pretreatment enhances the bioconversion of corn stover into ethanol
journal, January 2014

  • He, Yanqing; Zhang, Longping; Zhang, Jian
  • Biotechnology for Biofuels, Vol. 7, Issue 1
  • DOI: 10.1186/1754-6834-7-1

A highly efficient dilute alkali deacetylation and mechanical (disc) refining process for the conversion of renewable biomass to lower cost sugars
journal, January 2014

  • Chen, Xiaowen; Shekiro, Joseph; Pschorn, Thomas
  • Biotechnology for Biofuels, Vol. 7, Issue 1
  • DOI: 10.1186/1754-6834-7-98

Works referencing / citing this record:

Fiber fractionation to understand the effect of mechanical refining on fiber structure and resulting enzymatic digestibility of biomass
journal, January 2020

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High Titer Ethanol Production from Combined Alkaline/Alkaline Hydrogen Peroxide Pretreated Bamboo at High Solid Loading
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Nanomechanics of cellulose deformation reveal molecular defects that facilitate natural deconstruction
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